Magnetic engineering in InSe/black-phosphorus heterostructure by transition-metal-atom Sc-Zn doping in the van der Waals gap

Highlights: • Both the electronic and magnetic properties of InSe/BP heterostructure can be modulated effectively by the TM-atom dopants in the van der Waals gap. • The Sc-, Ti-, V-, Cr-, Mn- and Co-doped InSe/BP heterostructures exhibit the metallic states with non-zero magnetic moments, while Ni-, Cu- and Zn-doped cases retain the nonmagnetic semiconductor characteristics. • The half-metal properties are induced in the Fe-doped InSe/BP with magnetic moment of 2.0 μ_B and a high spin polarization of 100% at the Fermi level can be achieved. • The Sc-, Ti-, V-, Cr- and Mn-doped InSe/BP heterostructures have an antiferromagnetic coupling, whereas the Fe and Co doping result in weak ferromagnetic and paramagnetic coupling, respectively. Within the framework of the spin-polarized density-functional theory, we have studied the electronic and magnetic properties of InSe/black-phosphorus (BP) heterostructure doped with 3d transition-metal (TM) atoms from Sc to Zn. The calculated binding energies show that TM-atom doping in the van der Waals (vdW) gap of InSe/BP heterostructure is energetically favorable. Our results indicate that magnetic moments are induced in the Sc-, Ti-, V-, Cr-, Mn- and Co-doped InSe/BP heterostructures due to the existence of non-bonding 3d electrons. The Ni-, Cu- and Zn-doped InSe/BP heterostructures still show nonmagnetic semiconductor characteristics. Furthermore, in the Fe-doped InSe/BP heterostructure, the half-metal property is found and a high spin polarization of 100% at the Fermi level is achieved. The Cr-doped InSe/BP has the largest magnetic moment of 4.9 μ_B. The Sc-, Ti-, V-, Cr- and Mn-doped InSe/BP heterostructures exhibit antiferromagnetic ground state. Moreover, the Fe- and Co-doped systems display a weak ferromagnetic and paramagnetic coupling, respectively. Our studies demonstrate that the TM doping in the vdW gap of InSe/BP heterostructure is an effective way to modify its electronic and magnetic properties.